MATERIALS LETTERS
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2023
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IF 3
Zitong Wang,Haotian Wu,Yuan Fang,Hao Yang,Xiaomin Wang
The increasing drug resistance of bacteria due to the inappropriate use of various antibiotics has become an ongoing public health problem around the world. In this work, a novel Cu-hemin nanosheet with multilayer structure was synthesized by a simple green method. Integrating the peroxidase properties of hemin with the excellent photothermal conversion performance of IR780, the as-prepared Cu-hemin@IR780 can not only effectively catalyze hydrogen peroxide to produce reactive oxygen species (ROS), but also has a highly efficient and stable photothermal effect for sterilization. The antibacterial efficiency against MRSA can reach up to 98.96% by using chemodynamic therapy (CDT) and photothermal therapy (PTT) for synergistic sterilization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Tete Zhao,Xupeng Zong,Jiuding Liu,Jialei Chen,Keqiang Xu,Xiao Wang,Xijie Chen,Wutong Yang,Fangming Liu,Meng Yu,Fangyi Cheng
Copper-based nanomaterials are attractive in CO 2 electroreduction into valuable chemicals but still suffer from limited selectivity of C 2+ products due to the parasitic hydrogen evolution reaction and inefficient dimerization of absorbed CO intermediate (*CO). Herein, we report an in situ polymerization strategy to coat hydrophobic polymer containing methoxyl silane ((CH 3 O) 3 Si–) and trifluoromethyl (–CF 3 ) functional groups on Cu nanoparticles. The optimized Cu-poly exhibits a high Faradaic efficiency of 71.08 % and a remarkable partial current density of 355.4 mA cm −2 for C 2+ products in a membrane electrode assembly electrolyzer using a bicarbonate electrolyte. A combined study of density functional theory calculations and in situ infrared characterizations indicates that the enhanced performances could be ascribed to the decreased formation energy of *COCOH, induced by the withdraw-electron effect of –CF 3 and enhanced coverage of *CO. This work offers a new insight in tuning the electrocatalytic microenvironment through the surface polymerization process.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2023
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IF 7.8
Zibin Pan,Qingqiang Gao,Zuliang Chen
The elimination of arsenic (As) from arsenic-contaminated mine groundwater has become a worldwide problem because it causes environmental degradation and poses serious risks to human health. In this study, biosynthesized Fe/Cu nanoparticles (Fe/Cu NPs) were used for the simultaneous elimination of As(Ⅲ) and As(Ⅴ) from aqueous solution, resulting in their maximum amounts removed at 8.5 and 17.5 mg/g, respectively. SEM, FTIR, and XPS characterizations indicate that the Fe component on the Fe/Cu NPs acted as an adsorption and catalyst, while the Cu component mainly developed into a co-precipitation reaction with the As species, also facilitating the Fe catalytic processed. Meanwhile, adsorption isotherms , kinetics, and DFT calculations reveal that the removal of As(Ⅲ) was primarily physical/chemical adsorption and oxidation , while the elimination of As(Ⅴ) was co-precipitation and chemisorption. The most stable adsorption site, receiving 0.252 and 0.306 electrons from As(Ⅲ) and As(Ⅴ), respectively, was the unsaturated complexes of iron on the Fe/Cu NPs. Finally, the measurements and XPS results of Fe/Cu NPs in the treatment of groundwater show that the reduced capacity to remove As was attributed to a complex reaction system that disrupted the function of the Cu component, including co-precipitation and made the catalytic process possible. This explains there are differences in the reaction processes of biosynthetic Cu/Fe NPs in aqueous solution and groundwater.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Mingyi Liu,Hanchun Chen,Pengfei Xiao,Haodong Ji
Copper-manganese composite metal oxides (CuMnO y ) were prepared by hydrolysis-driven oxidation-reduction method and used to activate sulfite to degrade chlortetracycline hydrochloride (CTC) for the first time. The Jahn-Teller ions Mn 3+ and Cu 2+ exist in CuMnO y , which form a solid electric charge transport redox system and ensure the continuous generation of reactive oxygen species (ROS). Through the systematic study of the experimental parameters such as sulfite concentration, catalyst metal molar ratio, catalyst amounts and initial pH, the optimal degradation rate of CTC could reach 91.74% within 10 min and 94.46% after 30 min. The major reactive radicals were determined by radical quenching experiments and electron paramagnetic resonance (EPR) trapping techniques, and it was confirmed that SO 4 •- and •O 2 - played a nonnegligible role in the process of degrading CTC. Density functional theory (DFT) calculations show that higher Fukui indices ( f - and f 0 ) of CTC sites are more vulnerable to free radical attack. CuMnO y has low CTC degradation intermediate toxicity, high catalytic performance, good anti-interference ability, reusability and stability, and possesses decent application potential in the actual water treatment field.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Keliang Song,Zhipeng Liu,Aoshuang Yang,Yongsheng Li,Fangfang He,Zhuoni Jiang,Xiaoan Li,Zhengguo Chen,Wenbin Yang
Hydrated salt phase change materials (PCMs) have the advantages of high energy storage density and low cost, and have great application prospects in the field of phase change energy storage. However, the problems of supercooling, phase separation and leakage of hydrated salt PCMs limit their further applications. In this work, we designed and fabricated Cu-coated melamine foam (MF)/barium hydroxide octahydrate (BHO) shape-stabilized phase change materials (SSPCMs) with low supercooling. MF was used as supporting material and Cu as a nucleating agent and thermal conductivity enhancer by loading it onto MF via electroless plating . BHO was then encapsulated into the MF@Cu skeleton through vacuum impregnation to obtain BHO@MF@Cu SSPCMs. The results demonstrated that BHO@MF@Cu SSPCMs not only present very low supercooling degree of 0.12 °C and high thermal energy capacity of 247 J/g, but maintained a latent heat of phase transition of 229.3 J/g with little change in enthalpy after 100 thermal cycles. Moreover, compared to BHO, SSPCMs exhibited high thermal conductivity of 1.687 W m −1 K −1 , excellent shape stability, and thermal cycling stability. In summary, BHO@MF@Cu SSPCMs with low supercooling degree were prepared by electroless plating and vacuum impregnation in this study, which provides a new strategy to reduce the supercooling degree of hydrated salt PCMs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xiaojing Cui,Yequn Liu,Wenjun Yan,Yanfeng Xue,Yangang Mei,Jiamei Li,Xiaoqing Gao,He Zhang,Shanhui Zhu,Yulan Niu,Tiansheng Deng
Suppressing reverse water-gas-shift (RWGS) reaction is high desirable but challenging and underdeveloped for Cu/ZnO catalysts, particularly for commercial Cu/ZnO/Al 2 O 3 catalysts. Different from the current methodologies to reduce RWGS reaction, we report a simply surface silylation method for efficiently minimizing RWGS reaction over a commercial Cu/ZnO/Al 2 O 3 catalyst. This method suppresses STY CO (Space-time yield) from 97.4 to 0.7 g CO ·kg cat −1 ·h −1 , improving STY MeOH from 20.2 to 39.9 g MeOH ·kg cat −1 ·h −1 and methanol selectivity from 15.1 to 92.9 mol%. The combination of characterization methods and density functional theory calculations provide insight into the suppressing mechanism of surface silylation on catalyst. A hydroxyl (on ZnO)-promoted RWGS reaction cycle is discovered, which can be efficiently inhibited by the consuming of hydroxyls via surface silyation. Our results provide a way to regulate RWGS reaction on Cu/ZnO-based catalysts and are expected to the further use of silylation strategy to tune the interconversion of CO and CO 2 via RWGS/WGS reaction on hydrogenation catalysts.
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FUEL
·
2023
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IF 7.4
Xin Guo,Zhiyong Ding,Na Kang,Liu Yang,Yuanjiang Wang,Cheng Zhang,Zhaoqiang Li,Tiantian Zhang,Yan Wang,Yu Wang,Hao Qu
The zeolite-based catalyst is a promising option for the selective catalytic reduction (SCR) of nitrogen oxides (NO x ) due to its low toxicity. However, the challenge lies in its low-temperature activity. This study developed a multi-component catalytic system consisting of Ce/Mn/Cu-loaded Beta zeolite to reduce NO x . With fixed contents of Cu and Mn, we investigated the NH 3 -SCR process and the mechanism of action of the rare-earth species (i.e., Ce) in the system. Upon optimization of the content of Ce, the Ce/Mn/Cu-loaded Beta zeolite demonstrated enhanced low-temperature activity compared to samples loaded with Cu or Cu/Mn in the temperature range of 150–250 °C. When Ce was loaded in an appropriate proportion, it regulated the oxidation state of Cu, optimizing active adsorption species for NO and strengthening the strength of Brønsted acid sites in the catalyst. These synergetic effects led to improved NH 3 -SCR catalytic performance. This study can contribute to a better understanding of multiple metal-loaded zeolites in the NH 3 -SCR process and inform future design of Beta-type catalysts.
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ACS Applied Nano Materials
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2023
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IF 5.9
Jinqing He,Tong Dou,Shuteng Diao,Yiping Wang,Xuhui Zhao,Fazhi Zhang,Xiaodong Lei
The reduction of carbon dioxide to valuable chemical products is a hot topic of current research. In this article, Cu nanoparticle-decorated Fe3O4 (Cu/Fe3O4) is prepared by using layered double hydroxide (LDH) as the precursor. The CuFe-LDH is synthesized using the coprecipitation method and further reduced to obtain the final material Cu/Fe3O4. The uniform layered structure of LDH results in highly dispersed metallic elements in the corresponding Cu/Fe3O4, in which Cu atoms provide Cu0 and Cu+ pairs and good electrical conductivity during the reduction process with Fe3O4 as the framework. Therefore, Cu/Fe3O4 shows high selectivity for CO2 electroreduction to ethanol, in which the Faraday efficiency is 50.9% at −0.3 V vs RHE. Experimental results show that Cu/Fe3O4 generates uniformly distributed Cu+ sites during CO2 electroreduction, which is conducive to the formation of *CHO, a key intermediate to ethanol. This study provides a design method for catalysts of CO2 electroreduction with feasibility.
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Small
·
2023
·Vol. 19
·期 45
·2302022
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IF 13.3
Hai-Bing Zhao,Jia-Nan Huang,Qi Qin,Hong-Yan Chen,Dai-Bin Kuang
Rational design and facile synthesis of efficient environmentally friendly all-inorganic lead-free halide perovskite catalysts are of great significance in photocatalytic CO 2 reduction. Aiming at photogenerated charge carrier separation and CO 2 reaction dynamics, in this paper, a CsCuCl 3 /Cu nanocrystals (NCs) heterojunction catalyst is designed and synthesized via a simple acid-etching solution process by using Cu 2 O as the sacrificed template. Due to the disproportionation reaction of Cu 2 O induced by concentrated hydrochloric acid, Cu NCs can be deposited onto the surface of CsCuCl 3 microcrystals directly and tightly. As revealed by photoelectrochemical analysis, in situ Fourier transform infrared spectra, etc., the Cu NCs contribute a lot to extracting photoelectrons of CsCuCl 3 to improve the charge separation efficiency, regulating the CO 2 adsorption and activation, and also stabilizing the reaction intermediates. Therefore, CsCuCl 3 /Cu heterojunction exhibits a total electron consumption rate of 58.77 µmol g −1 h −1 , which is 2.9-fold of that of single CsCuCl 3 . Moreover, high CH 4 selectivity of up to 92.7% is achieved, which is much higher than that of CsCuCl 3 (50.4%) and most lead-free halide perovskite-based catalysts. This work provides an ingenious but simple strategy to rationally design cocatalysts in situ decorated perovskite catalysts for manipulating both the catalytic activity and the product selectivity.
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Engineering
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2023
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IF 12.8
Ning Li,Haoxi Dai,Mengting He,Jun Wang,Zhanjun Cheng,Beibei Yan,Wenchao Peng,Guanyi Chen
The distribution pattern of metals as active centers on a substrate can influence the peroxymonosulfate (PMS) activation and contaminants degradation. Herein, atomic layer deposition is applied to prepare Cu single atom (SA-Cu), cluster (C-Cu), and film (F-Cu) decorated MXene catalysts by regulating the number of deposition cycles. In comparison with SA-Cu-MXene (adsorption energy ( E ads ) = −4.236 eV) and F-Cu-MXene ( E ads = −3.548 eV), PMS is shown to adsorb preferably on the C-Cu-MXene surface for activation ( E ads = −5.435 eV), realizing higher utilization efficiency. More SO 4 − · are generated in C-Cu-MXene/PMS system with steady-state concentration and 1–3 orders of magnitude higher than those in the SA-Cu-MXene and F-Cu-MXene activated PMS systems. Particularly, the contribution of SO 4 − · oxidation to sulfamethoxazole (SMX) degradation followed the order, C-Cu-MXene (97.3%) > SA-Cu-MXene (90.4%) > F-Cu-MXene (71.9%), realizing the larger SMX degradation rate in the C-Cu-MXene/PMS system with the degradation rate constants ( k ) at 0.0485 min −1 . Additionally, SMX degradation routes in C-Cu-MXene/PMS system are found with fewer toxic intermediates. Through this work, we highlighted the importance of guided design of heterogeneous catalysts in the PMS system. Appropriate metal distribution patterns need to be selected according to the actual water treatment demand. Metal sites could be then fully utilized to produce specific active species to improve the utilization efficiency of the oxidants.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Shubin Cheng,Qian Lei,Coner Deng,Weixin Lei,Honglin Chen
A green protocol for refining industrial chemicals containing formaldehyde (FA) impurities is presented here for the first time. FA, as an unreactant or a byproduct, causes separation problems in many industrial processes. It can be removed to a level of less than 1 ppm with easily separable methanol formation using commercial Cu/ZnO/Al 2 O 3 catalyst at atmospheric pressure in the absence of external hydrogen. The formation of methanol is achieved by the transfer of hydrogen species generated with the assistance of water to free FA, affording high methanol selectivity (62 %). By investigating potential intermediates and implementing deuterium labeling experiments, together with carbon and hydrogen balance calculations, a plausible pathway of water-assisted FA removal is proposed. Moreover, the in situ generated hydrogen species can be transferred directly into unsaturated compounds for selective reduction.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Donglin Yang,Bingxiao Feng,Yaping Liu,Chaoting Deng,Hengjun Gai,Meng Xiao,Tingting Huang,Quanhong Zhu,Hongbing Song
The manner of ammonia-containing wastewater in industrial production has always been an urgent issue that needs to be solved. Accordingly, a carbon-supported low-loading Ru/Cu bimetallic catalyst with high activity and hydrothermal stability was produced through facile disposal for catalytic wet air oxidation (CWAO). In the preparation process, Ru and Cu ions were loaded onto micro mesoporous carbon prepared through the calcination of potassium citrate by impregnation. Various characteristic techniques were utilized to characterize their structures and morphology, and results show that the calcination temperature with micro-mesopores’ characteristics could regulate the morphology of carbon. The results of catalytic experiments demonstrated that the obtained catalyst showed excellent catalytic performance in the process of CWAO. The Ru/Cu@C-700 catalyst achieved 99.6 % conversion of ammonia water at 800 ppm and 99.1 % selectivity to nitrogen at 200 °C and 2 MPa O 2 in 4 h. The ammonia nitrogen content in the treated water was less than 15 ppm, meeting the standard for direct discharge . Moreover, no apparent deactivation phenomenon was observed after five cycles, indicating that the prepared catalyst can effectively prevent the leaching of ruthenium and copper nanoparticles . The low loading (less than 1 %) of the Ru/Cu bimetallic catalyst can significantly reduce costs and can synergistically enhance conversion and selectivity, providing an effective strategy for studying the CWAO of ammonia.
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